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Vol. 14 (2022)

Insights Into the Interfacial Degradation of High-Voltage All-Solid-State Lithium Batteries

https://doi.org/10.1007/s40820-022-00936-z
Jiawen Li
School of Advanced Material, Peking University Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China
Yuchen Ji
School of Advanced Material, Peking University Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China
Haoran Song
School of Advanced Material, Peking University Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China
Shiming Chen
School of Advanced Material, Peking University Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China
Shouxiang Ding
School of Advanced Material, Peking University Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China
Bingkai Zhang
Guangzhou Key Laboratory of Clean Transportation Energy Chemistry, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 51006, People’s Republic of China
Luyi Yang
School of Advanced Material, Peking University Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China
Yongli Song
School of Advanced Material, Peking University Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China
Feng Pan
School of Advanced Material, Peking University Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China

Corresponding Author: Feng Pan

panfeng@pkusz.edu.cn

Nano-Micro Letters, Vol. 14 (2022), Article Number: 191

Abstract

Poly(ethylene oxide) (PEO)-based solid polymer electrolyte (SPE) is considered as a promising solid-state electrolyte for all-solid-state lithium batteries (ASSLBs). Nevertheless, the poor interfacial stability with high-voltage cathode materials (e.g., LiCoO2) restricts its application in high energy density solid-state batteries. Herein, high-voltage stable Li3AlF6 protective layer is coated on the surface of LiCoO2 particle to improve the performance and investigate the failure mechanism of PEO-based ASSLBs. The phase transition unveils that chemical redox reaction occurs between the highly reactive LiCoO2 surface and PEO-based SPE, resulting in structure collapse of LiCoO2, hence the poor cycle performance of PEO-based ASSLBs with LiCoO2 at charging voltage of 4.2 V vs Li/Li+. By sharp contrast, no obvious structure change can be found at the surface of Li3AlF6-coated LiCoO2, and the original layered phase was well retained. When the charging voltage reaches up to 4.5 V vs Li/Li+, the intensive electrochemical decomposition of PEO-based SPE occurs, leading to the constant increase of cell impedance and directly causing the poor performance. This work not only provides important supplement to the failure mechanism of PEO-based batteries with LiCoO2, but also presents a universal strategy to retain structure stability of cathode–electrolyte interface in high-voltage ASSLBs.


Highlights:


1 The cycle performance of poly(ethylene oxide) (PEO)-based all-solid-state lithium batteries with LiCoO2 cathode was greatly improved via coating LiCoO2 with high-voltage stable Li3AlF6.
2 At the upper cutoff voltage of 4.2 V, the poor electrochemical performance is mainly originated from the structure collapse of LiCoO2 at the surface instead of the decomposition of PEO.
3 When the voltage reaches 4.5 V or even higher potentials, the intensive electrochemical decomposition of PEO-based solid polymer electrolyte accelerated interfacial degradation.

Keywords

Solid-state battery Poly(ethylene oxide) Surface modification Interface stability High-voltage cathode
Li, Jiawen, Yuchen Ji, Haoran Song, Shiming Chen, Shouxiang Ding, Bingkai Zhang, Luyi Yang, Yongli Song, and Feng Pan. 2022. “Insights Into the Interfacial Degradation of High-Voltage All-Solid-State Lithium Batteries”. Nano-Micro Letters 14 (September):191. https://doi.org/10.1007/s40820-022-00936-z.
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